Gamma-Ray Transitions Induced in Nuclear Spin Isomers by X-Rays

Because of the high density of energy storage and the large cross section for its release, nuclear spin isomers have attracted considerable recent interest. The triggering of induced gamma emission from them has encouraged efforts to develop intense sources of short-wavelength radiation. One of the more interesting examples is the 16⁺ 4-qp isomer of ¹⁷⁸Hf which stores 2.445 MeV for a half-life of 31 years meaning that as a material, such isomeric ¹⁷⁸Hf would store 1.3 GJ/g. Recently, a sample containing 6.3×10¹⁴ nuclei of the isomer of ¹⁷⁸Hf was irradiated with X-ray pulses derived from a device operated at 15 mA to produce bremsstrahlung radiation with end point energies set to values between 60 and 90 keV. Emission of gamma radiation from the sample was increased by 1–2% above the quiescent value of spontaneous emission. Such an accelerated decay of the ¹⁷⁸Hf isomer is consistent with an integrated cross section of 2.2×10⁻²² cm² keV if the resonant absorption of the X-rays takes place below 20 keV as indicated by the use of selective absorbing filters in the irradiating beam. The work reported here describes the current experimental focus and results recently obtained with the use of coincident detection of emitted gamma photons by several detectors. This revised version was published online in July 2006 with corrections to the Cover Date.     

Non-Linear Excitation and Decay of Low-Energy Nuclear Isomers Produced under Femtosecond Laser–Plasma Interaction

The properties of internal electronic conversion of nucleus excited in hot dense laser plasma are considered. The important role of dynamics of plasma charge state in residual gas is shown. We are also considering the role of multi-quanta photoexcitation of low-energy nuclear levels in this plasma. This revised version was published online in August 2006 with corrections to the Cover Date.     

Nuclear Level Density at High Spin and Excitation Energy

The intensive studies of equilibrium processes in heavy-ion reaction have produced a need for information on nuclear level densities at high energies and spins. The Fermi gas level density is often used in investigation of heavy-ion reaction studies. Some papers have claimed that nuclear level densities might deviate substantially from the Fermi gas predications at excitations related to heavy-ion reactions. The formulae of calculation of the nuclear level density based on the theory of superconductivity are presented, special attention is paid to the dependence of the level density on the angular momentum. The spin-dependent nuclear level density is evaluated using the pairing interaction. The resulting level density for an average spin of 52 ħ is evaluated for ¹⁵⁵Er and compared with experimental data. Excellent agreement between experiment and theory is obtained.     

强激光场中对称三原子分子多光子振动激发的动力学李代数计算

用分子的内坐标给出的动能加上用动力学代数方法给出的用内坐标表示的分子势能得出对称三原子分子的总的能量表达式,给出了时间演化算子并计算了对称三原子分子在强激光场中振动激发.作为例子,计算了H2O分子在频率wF=3652 cm-1的激光场中的激发,通过讨论可以发现H2O在激光场中的跃迁几率随时间的变化是周期性的,水分子从激光场中吸收的能量由吸收的平均光子数确定,被吸收的平均光子数随时间的变化也是周期性的.     

强激光场中对称三原子分子多光子振动激发的动力学李代数计算

用分子的内坐标给出的动能加上用动力学代数方法给出的用内坐标表示的分子势能得出对称三原子分子的总的能量表达式,给出了时间演化算子并计算了对称三原子分子在强激光场中振动激发。作为例子,计算了H2O分子在频率 的激光场中的激发,通过讨论可以发现H2O在激光场中的跃迁几率随时间的变化是周期性的,水分子从激光场中吸收的能量由吸收的平均光子数确定,被吸收的平均光子数随时间的变化也是周期性的。     

核自旋单重态的制备及其转化效率和寿命的影响因素分析

长寿命核自旋单重态（LLS）因具有寿命较长这一特性而具有广泛的应用前景.本文在一个三肽样品（alanylglycylgcine,AGG）的水溶液中,对结构中离手性碳较远的二自旋体系进行核自旋单重态的制备,并探究了样品浓度、温度、射频发射中心位置、自旋体系之间的J耦合常数,以及磁场不均匀性五个因素对LLS的转化效率及其寿命的影响.实验结果表明,核自旋单重态的转化效率和寿命均不受样品浓度以及磁场不均匀性的影响.寿命会随实验温度的升高不断增加,转化效率随温度的下降而减小.射频中心位置在小范围内变化时,核自旋单重态制备所受影响不明显;但当变化较大时,其转化效率与寿命明显减小.同时,核自旋单重态对J耦合的变化则比较敏感,当J值选择不精准时,转化效率及寿命都出现明显降低.     

Anomalous Ortho-to-Para Ratio of Nuclear Spin Isomers of H2O at Low Temperatures

A theoretical model proposed for nuclear spin isomers of H₂O molecules located inside the C₆₀ fullerene explains an anomalously high stability of ortho-H₂O isomers detected in the experiments reported in [B. Meier et al., Nature Commun. 6, 8112 (2015)] at a temperature of T = 5 K.

     

Relaxation Processes at High Levels of Vibrational Excitation of Polyatomic Molecules in the Ground Electronic State

By the spectral and kinetic characteristics of the luminescence of vapors of polyatomic molecules (anthracene, anthraquinone, fluorenone) initiated by selective IR multiphoton excitation (IR MPE) of molecules in the ground electronic state S ₀ the relaxation processes proceeding under vibrational excitation of molecules to energies exceeding the energies of the lower excited electronic states have been investigated. The changes in the spectral and kinetic characteristics with increasing CO₂ laser energy density and vapor P _v and foreign gas pressure P _FG are analyzed. They are similar to the characteristics obtained for normal fluorescence of these molecules with changing vibrational energy E _vib content. On the basis of experimental data and model calculations it has been concluded that at the laser radiation densities used in the case of IR MPE the molecules reach energies considerably exceeding the energies of the electronic levels. It is shown that a nonadiabatic connection between the electronic states leads to the population of mixed electronic states isoenergetic to the vibrational levels of the ground electronic state and to emission of delayed luminescence spectrally identical to the normal luminescence of these molecules. It has been found that when high vibrational levels are populated, new relaxation channels, such as reverse electron relaxation, emission from high vibrational levels of the ground electronic state, and multiquantum vibrational energy transfer at collisions leading to a rapid establishment of vibrational equilibrium become important.     

Transient Absorption of Organic Molecules under High-Power Laser Excitation

In the present work, results of investigations into the transient absorption of some organic compounds by the method of pulsed flash photolysis are given. Experimental investigations were carried out using an original setup of pulsed flash photolysis with an exciting pulse of XeCl-laser radiation of nanosecond duration and sensing by broadband laser-transient fluorescent radiation of a mixture of organic fluorophors called “white light” excited by the same source in the wavelength range 330–750 nm. The setup registers the short-living (singlet-singlet) and long-living (triplet-triplet) absorptions. The transient absorption spectra of already investigated para-terphenyl, naphthalene, and 1-phenyl-2(2-naphthyl)-ethylene molecules are presented; the spectra of the transient absorption and its nature are in good agreement with the experimental and calculated data published in the literature. We first investigated the transient absorption of LOC1 (S₁-S_n at 580 nm and T₁-T_n at 500 nm) and phenalemine 512 (S₁-S_n at 395 nm). It is demonstrated that the experimentally observed induced absorption of phenalemine 512 and PD 789 is the S₁-S_n absorption, which is in good agreement with the results of quantum-chemical calculations. __________ Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 9, pp. 12–16, September, 2005.     

Influence of Vibrational Excitation of Triplet Molecules of Anthraquinone on the Photochemical Processes in Gas Mixtures with Amines

By the quenching of the delayed fluorescence (DF) of anthraquinone vapors by aliphatic amines (diethylamine, dibutylamine, cyclohexylamine) and pyridine the photoinduced processes proceeding with the participation of vibrationally excited triplet molecules of anthraquinone have been investigated. The DF quenchingrate constants K _q varying from 1·10⁶ sec^–1·torr^–1 in mixtures with diethylamine to 7·10³ sec^–1·torr^–1 in mixtures with pyridine have been estimated. A correlation between the values of K _q and the ionization potentials of foreign gases confirming the important role of interactions with charge transfer in the quenching of triplet molecules in the gas phase has been established. The influence of other relaxation processes on the DF quenching is considered. It is shown that the intermolecular vibrational relaxation in the T ₁ triplet state leading to the establishment of relaxation equilibrium at a vibrational temperature T _vib considerably increasing the medium temperature is the fastest process among the biomolecular processes (rate constants K _col ^V > 10⁶ sec^–1·torr^–1 > K _q). The values of T _vib and the vibrational energies E _vib of the triplet molecules after the energy exchange in the collisional complex have been estimated. It has been concluded that the photochemical reaction yield is determined by the intermolecular processes proceeding in the T ₁ state at a vibrational equilibrium characterized by high values of T _vib. The influence of E _vib of triplet molecules on the DF quenching rates at a photoinduced electron transfer is considered.     

Effect of Excitation and Vibrational Temperature on the Dissociation of Nitrogen Molecules in Ar-N2 Mixture RF Discharge

Non-equilibrium argon-nitrogen mixture plasma generated at 13.56 MHz is characterized by optical emission spectroscopy and Langmuir probe techniques. The excitation and vibrational temperature are studied as a function of argon percentage in the mixture, at 30-Pa filling pressure and input RF powers of 200 and 300 watt, to find out their role in dissociation of N₂ molecules. In this work, the excitation temperature is determined from Ar-I emission line intensities by using the simple Boltzmann plot method and is found to increase with argon mixing in nitrogen plasma. In similar fashion, the vibrational temperature of second positive system has been determined and is found to also have increasing trend with argon addition. The effect of excitation and vibrational temperature on the nitrogen molecular dissociation level is also monitored. It is observed that N/N ₂ ratio increases with increase in excitation and vibrational temperature and falls slightly at the end.     

Photophysical Processes in the Gas Phase at High Levels of Vibrational Excitation of Triplet Molecules of Benzophenone and Fluorenone

By the delayed fluorescence activated by direct multiphoton excitation of triplet molecules by CO₂–laser radiation we have studied the prevailing deactivation pathways of triplet molecules with a high store of vibrational energy E _vib. The dependences of the kinetic characteristics of delayed fluorescence on the presence of vapors and foreign gases have been used to estimate the rates and efficiencies of intermolecular vibrational relaxation in the vibrational quasi–continuum of the triplet state T ₁. By the changes in the intensities and decay rates over a wide range of vibrational energies we have established the E _vib dependences of reversible intercombination conversion between the states T ₁ and S ₁ and interconversion from T ₁ to the ground electronic state S ₀ for both the case of isolated excited molecules and at a steady vibrational temperature. It is shown that at high vibrational temperatures the radiationless transition from the T ₁ state to S ₀ has an activation character and is accomplished through the energy barrier. The conditions for going to an exponential dependence have been determined. It has been found that the obtained dependences are in good agreement with the known experimental results. The influence of molecular and environmental characteristics on the decay rate of triplet molecules is compared.     

Anharmonic Potential Functions in Polyatomic Molecules as Derived from Their Vibrational and Rotational Spectra

It is well known that the anharmonic part of the molecular potential function contributes to the vibration-rotation energy and to the apparent molecular geometry, although the anharmonic effect is not so profound as that from its harmonic counterpart. Nevertheless, it cannot simply be ignored for the precise treatment of molecular dynamics and structures. For a better understanding of the molecular potential function, it is highly desirable to extend the force constant calculation to evaluate the terms beyond quadratic, which will give a more realistic potential map of polyatomic molecules for wider ranges of atomic displacements. The vibrational anharmonicity also affects the transition intensities through the mixing vibration-rotation wave functions.     

Non-Radiative Triggering of Long-Lived Nuclear Isomers

The triggering of long-lived isomeric nuclei by non-radiative excitation to a relatively short-lived mediating state is considered. Coulomb triggering in inelastic scattering of heavy ions, a transfer of triggering energy from resonant electron transitions of atomic shell (NEET) and triggering by capture of a free electron into a bound atomic state (NEEC) are discussed. Cross sections for the above processes of non-radiative triggering are presented and the relative efficiencies of these different triggering mechanisms are discussed. Numerical estimates are presented for the selected isomers. This revised version was published online in August 2006 with corrections to the Cover Date.     

Intermolecular Vibrational Relaxation in Mixtures of Excited Benzophenone and Anthraquinone Molecules with Water Vapor

The intermolecular vibrational energy transfer from triplet molecules of benzophenone and anthraquinone to H₂O molecules has been investigated. To determine the rates of establishment of vibrational (V-V) and thermal (V-T) equilibrium in a vibrational quasi-continuum of mixed singlet-triplet levels, the dependences of the decay rates and intensities of the fast and slow components of delayed fluorescence on the H₂O vapor pressure have been investigated. For V-V relaxation, the efficiencies ₁ and the mean energies E transferred per collision in mixtures with H₂O and other polyatomic foreign gases have been compared. It has been established that the efficiencies ₁ for quasi-resonant vibrational energy transfer (V-V) from benzophenone and anthraquinone to H₂O are an order of magnitude lower than the gas-kinetic ones and lower than those obtained under the same experimental conditions for such foreign gases as C₅H₁₂, SF₆, and CCl₄, and decrease with increasing temperature in the 433–513 K range. It has been concluded that the mechanism of V-V relaxation in mixtures with H₂O are determined by long-range attractive forces. In mixtures with H₂O, no acceleration of V-T relaxation due to the formation of hydrogen bonds has been revealed. The low-efficiency thermalization process (V-T relaxation) is controlled by short-range repulsive forces, and the differences between the intensities ₂ for mixtures of benzophenone and anthraquinone with H₂O and other polyatomic gases are determined by the change in the reduced mass of interacting molecules.     

Vibrational Mean Amplitudes of XY3 Pyramidal Molecules

The vibrational mean amplitudes for bonded as well as for nonbonded distances have been evaluated for AsP₃, SbP₃, and PAs₃ at temperatures : T = 0^oK, T = 298.15^oK and T=500 ^oK using recent vibrational data. The results have been briefly discussed.     

The Gamma Resonance Problem of Long-Lived Nuclear Isomers

A review is given of the studies relating to the problem of γ-resonant (Mössbauer) excitation of long-lived nuclear isomers. The theoretical estimates of possible γ-line broadening are presented. Earlier experiments are described with ^107mAg and ^109mAg isomers using polycrystalline samples of pure Ag and Ag-Pd alloys. The results of these experiments did not contradict the theoretical predictions. The series of papers using Ag single-crystal γ-sources is reviewed. Their results were interpreted as indications of a rather small ^109mAg γ-line broadening, which cannot be explained by modern theory. The results of the last experiments by ITEP group with ^109mAg are also presented. These data may be coordinated with results of other research, if one takes into account the Zeeman splitting of the γ-spectra by Earth's magnetic field.